气候变化领域集成服务门户(CCPortal): Carboxylate anion generation in aqueous solution from carbonate radiolysis, a potential route for abiotic organic acid synthesis on Earth and beyond

CCPortal

DOI	10.1016/j.epsl.2021.116892
	Carboxylate anion generation in aqueous solution from carbonate radiolysis, a potential route for abiotic organic acid synthesis on Earth and beyond
	Vandenborre J.; Truche L.; Costagliola A.; Craff E.; Blain G.; Baty V.; Haddad F.; Fattahi M.
发表日期	2021
ISSN	0012821X
卷号	564
英文摘要	Low molecular weight carboxylate anions such as formate (HCOO−), acetate (CH3COO−) and oxalate (C2O42−) have been shown to play an important role in supporting deep subsurface microbial ecosystems. Their origin whether biological or abiotic is currently highly debated, but surprisingly radiolytic production has rarely been considered, as it is the case for H2. Here, we address this question through dedicated irradiation experiments. Aqueous solutions containing carbonate, formate, acetate or oxalate have been irradiated using both the 60.7 MeV α-beam of the ARRONAX cyclotron (Nantes, France) and 661.7 keV γ-Ray in order to reveal the mechanism and chemical yield of radiation-induced dissolved carbonate degradation. The yields (G-values) of carboxylate anions production/degradation in low-concentration carbonate solution (0.01 to 1 mmol L−1) are measured. Carbonate degradation occurs through three consecutive steps (Carbonate →I Formate →II Acetate →III Oxalate) involving formate radical (CO2−•), dihydrogen (H2), and carbon dioxide (CO2) generation. Dissolved carbonate radiolysis provides a consistent pathway for both enhancing two-fold the radiolytic H2 production compared to pure water and generating carboxylic species, chiefly oxalate, readily available for microbes. Radiation-induced carbonate degradation may produce substantial amount (millimolar concentration) of carboxylate anions in ancient groundwaters from deep crystalline bedrocks. Subsurface lithoautotrophic microbial ecosystems may not only be supported by radiolytic H2 but also by carboxylate species from carbonate radiolysis. Carbonate radiolysis can be also an endogenous source of carboxylate species on Mars and other planetary bodies. © 2021 Elsevier B.V.
关键词	acetate carbon cycling chemical yield deep biosphere formate oxalate
英文关键词	Carbon dioxide; Carbonation; Carboxylation; Gamma rays; Groundwater; Hydrogen production; Negative ions; Petroleum tar; Radiation chemistry; Radiolysis; Acetate; Carbon cycling; Carboxylate anions; Chemical yields; Deep biosphere; Formate; Low molecular weight; Organics; Radiation-induced; Subsurface microbial ecosystems; Oxalic acid; abiotic factor; acetate; anion; aqueous solution; biosphere; carbon cycle; carbonate; organic acid; oxalate
语种	英语
来源期刊	Earth and Planetary Science Letters
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/203318
作者单位	Subatech, UMR 6457, Institut Mines-Télécom Atlantique, CNRS/IN2P3, Université de Nantes, 4, Rue Alfred Kastler, La chantrerie BP 20722, 44307, Nantes cedex 3, France; GIP ARRONAX, 1 rue ARRONAX, CS 10112, Saint-Herblain Cedex, 44817, France; University Grenoble Alpes, CNRS, ISTerre, CS 40700, Grenoble, 38058, France
推荐引用方式 GB/T 7714	Vandenborre J.,Truche L.,Costagliola A.,et al. Carboxylate anion generation in aqueous solution from carbonate radiolysis, a potential route for abiotic organic acid synthesis on Earth and beyond[J],2021,564.
APA	Vandenborre J..,Truche L..,Costagliola A..,Craff E..,Blain G..,...&Fattahi M..(2021).Carboxylate anion generation in aqueous solution from carbonate radiolysis, a potential route for abiotic organic acid synthesis on Earth and beyond.Earth and Planetary Science Letters,564.
MLA	Vandenborre J.,et al."Carboxylate anion generation in aqueous solution from carbonate radiolysis, a potential route for abiotic organic acid synthesis on Earth and beyond".Earth and Planetary Science Letters 564(2021).